Wang Guangming, Chen Shunhua, Duan Qiwei, Wei Fenfei, Lin Sen, Xie Zailai
Key Laboratory of Advanced Carbon-Based Functional Materials, Fujian Province University), State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, 2 Xueyuan Road, 350016, Fuzhou, China.
Angew Chem Int Ed Engl. 2023 Sep 18;62(38):e202307470. doi: 10.1002/anie.202307470. Epub 2023 Aug 9.
Borocarbonitride (BCN) materials are newly developed oxidative dehydrogenation catalysts that can efficiently convert alkanes to alkenes. However, BCN materials tend to form bulky B O due to over-oxidation at the high reaction temperature, resulting in significant deactivation. Here, we report a series of super stable BCN nanosheets for the oxidative dehydrogenation of propane (ODHP) reaction. The catalytic performance of the BCN nanosheets can be easily regulated by changing the guanine dosage. The control experiment and structural characterization indicate that the introduction of a suitable amount of carbon could prevent the formation of excessive B O from BCN materials and maintain the 2D skeleton at a high temperature of 520 °C. The best-performing catalyst BCN exhibits 81.9 % selectivity towards olefins with a stable propane conversion of 35.8 %, and the propene productivity reaches 16.2 mmol h g , which is much better than hexagonal BN (h-BN) catalysts. Density functional theory calculation results show that the presence of dispersed rather than aggregated carbon atoms can significantly affect the electronic microenvironment of h-BN, thereby boosting the catalytic activity of BCN.
硼碳氮化物（BCN）材料是新开发的氧化脱氢催化剂，能够有效地将烷烃转化为烯烃。然而，由于在高反应温度下过度氧化，BCN材料容易形成大量的B-O，导致显著失活。在此，我们报道了一系列用于丙烷氧化脱氢（ODHP）反应的超稳定BCN纳米片。通过改变鸟嘌呤用量，可以轻松调节BCN纳米片的催化性能。对照实验和结构表征表明，引入适量的碳可以防止BCN材料形成过量的B-O，并在520℃的高温下维持二维骨架结构。性能最佳的催化剂BCN对烯烃的选择性为81.9%，丙烷转化率稳定在35.8%，丙烯产率达到16.2 mmol h-1 g-1，远优于六方氮化硼（h-BN）催化剂。密度泛函理论计算结果表明，分散而非聚集的碳原子的存在会显著影响h-BN的电子微环境，从而提高BCN的催化活性。
